The role of diffusion in the nucleation of calcium carbonate

Abstract

Both simulation and experimental results confirmed the significance of chemical diffusion in the nucleation of calcium carbonate, which was ascribed to the enhancement of unit collision driven by diffusion. Nucleation widely exists in nature, from cloud formation to haze generation. The classical nucleation theory (CNT) was created to describe the nucleation process, but it fails to predict many experimental phenomena due to the short consideration of nanoscale phenomena and macroscale dynamics. Although the attachment and detachment of monomers are considered in the developed model of nucleation, the diffusion of chemicals in the bulk is not valued as supersaturation in the nucleation process so far. Here we employ simulation and experimental approaches to investigate how the diffusion of ions affects the nucleation of calcium carbonate. The diffusion of ions is regulated by the viscosity of solvents and the sonication imposed on the solution. It is found that the nucleation rates increased exponentially with the diffusion coefficient of ions, which is beyond the prediction of CNT. This abnormal finding might be ascribed to the involvement of cluster aggregation in the nucleation of calcium carbonate. This study highlights the significance of chemical diffusion in the nucleation process, which may help to revise the nucleation theory and develop solutions for the rational synthesis of materials, as well as for the control of air pollution.